通过S型ZnInS/ZnO异质结光生电荷的空间分离实现高效光催化产氢
Efficient photocatalytic hydrogen production by space separation of photo-generated charges from S-scheme ZnInS/ZnO heterojunction.
作者信息
Xie Ziyu, Xie Linjun, Qi Fangfang, Liu Haizhen, Meng Lingyi, Wang Jiangli, Xie Yiming, Chen Jing, Lu Can-Zhong
机构信息
Engineering Research Center of Environment-Friendly Functional Materials, Ministry of Education, Institute of Materials Physical Chemistry, Huaqiao University, Xiamen 361021, China; CAS Key Laboratory of Design and Assembly of Functional Nanostructures, and Fujian Provincial Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China; Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials, Xiamen Institute of Rare-earth Materials, Haixi Institutes, Chinese Academy of Sciences, Xiamen 361021, China.
CAS Key Laboratory of Design and Assembly of Functional Nanostructures, and Fujian Provincial Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China; Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials, Xiamen Institute of Rare-earth Materials, Haixi Institutes, Chinese Academy of Sciences, Xiamen 361021, China.
出版信息
J Colloid Interface Sci. 2023 Nov 15;650(Pt A):784-797. doi: 10.1016/j.jcis.2023.07.032. Epub 2023 Jul 7.
ZnInS/ZnO heterostructures have been achieved by a simple in-situ growth solvothermal method. Under full spectrum irradiation, the optimal photocatalyst 2ZnInS/ZnO exhibits H evolution rate of 13,638 (water/ethanol = 1:1) and 3036 (water) μmol·gh, which is respectively 4 and 5 times higher than that of pure ZnInS. In situ illumination X-ray photoelectron spectroscopy (ISI-XPS) analysis and density functional theory (DFT) calculations show that the electrons of ZnInS are removed to ZnO through hybridization and form an internal electric field between ZnInS and ZnO. The optical properties of the catalyst and the effect of internal electric field (IEF) can increase photo-generated electrons (e)-holes (h) transport rate and enhance light collection, resulting in profitable photocatalytic properties. The photoelectrochemical and EPR results show that a stepped (S-scheme) heterojunction is formed in the ZnInS/ZnO redox center, which greatly promotes separation of e-h pairs and efficient H evolution. This research offers an effective method for constructing an efficient S-Scheme photocatalytic system for H evolution.
通过一种简单的原位生长溶剂热法制备了ZnInS/ZnO异质结构。在全光谱照射下，最佳光催化剂2ZnInS/ZnO的析氢速率在水/乙醇 = 1:1时为13638 μmol·g⁻¹h⁻¹，在水中为3036 μmol·g⁻¹h⁻¹，分别比纯ZnInS高4倍和5倍。原位光照X射线光电子能谱（ISI-XPS）分析和密度泛函理论（DFT）计算表明，ZnInS的电子通过杂化转移到ZnO上，并在ZnInS和ZnO之间形成内建电场。催化剂的光学性质和内建电场（IEF）的作用可以提高光生电子（e⁻）-空穴（h⁺）的传输速率并增强光捕获能力，从而产生良好的光催化性能。光电化学和电子顺磁共振结果表明，在ZnInS/ZnO氧化还原中心形成了阶梯型（S型）异质结，这极大地促进了e⁻-h⁺对的分离和高效析氢。该研究为构建用于析氢的高效S型光催化体系提供了一种有效方法。
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